Chemically synthesized NPs display a great diversity of polyhedral shapes [1]}. Recent experiments revealed that under attractive interactions from van der Waals forces, hydrogen bonds, and coordination bonds, these NPs can form a number of assemblies with interesting structural order, high complexity, and hierarchy at the nanoscale, from helices to curved platelets, capsids, and hedgehogs  [2]}, [3]}, [4]}, [5]}, [6]}, [7]}, [8]}, [9]}, [10]}, [11]}. How these simple polyhedral building blocks led to the observed complex structures remains an open fundamental question. Simulations of these systems face challenges from both the intrinsic complexity of NP-NP interactions and the rugged free-energy landscape of the high-dimensional phase space of their assembly [12]}, [13]}.
Real-time imaging techniques have only recently begun to reach the resolution to investigate the pathways of these self-assembly problems [14]}, [15]}.
The answer to this question is not only important for emerging technologies stemming from the unique properties of these nanoscale assemblies, but also offers new insight into how complex hierarchical structures form in nature.
